Here is an example from one of my classes
DataRelation relBookingMNI;
relBookingMNI = new DataRelation("BookingToBookingMNI",dsBooking.Tables["Booking"].Columns["Record_Id"],dsBooking.Tables["Booking_MNI"].Columns["booking_record_id"]);
dsBooking.Relations.Add(relBookingMNI);
dsBooking is my main dataset that contains 2 tables. Reservation and reservation_MNI If Record_Id is the primary key and reserve_record_id is the foreign key
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DataTable dtBooking = ds.Tables[0];
DataTable dtBooking_MNI = ds.Tables[1];
dtBooking.PrimaryKey = new DataColumn[] {dtBooking.Columns["Record_Id"]};
dtBooking_MNI.PrimaryKey = new DataColumn[] {dtBooking_MNI.Columns["booking_Record_Id"]};
DataColumn[] dcBookingColsArray = new DataColumn[1] {dtBooking.Columns["Record_Id"]};
DataColumn[] dcBookingMNIColsArray = new DataColumn[1] {dtBooking_MNI.Columns["booking_record_Id"]};
DataRelation relBooking_To_MNI = new DataRelation("Booking_To_MNI",dcBookingColsArray,dcBookingMNIColsArray);
ds.Relations.Add(relBooking_To_MNI_Units);
grdBooking.DataSource = ds;